期刊
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
卷 23, 期 35, 页码 19854-19861出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/d1cp02787e
关键词
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资金
- National Natural Science Foundation of China [21903025, 21825301]
- National Key Research and Development Program of China [2018YFA0208602]
This study investigates the promotional effect of oxygen vacancies on photoelectron transfer in TiO2, showing that ionized oxygen vacancies play a crucial role in photocatalysis, especially in the rutile phase. The results indicate that certain ionized oxygen vacancies patterns can enhance the photocatalytic efficiency of TiO2.
Oxygen vacancies (O-v) are widely considered to play crucial roles in photocatalysis, but how and why they contribute to improved performances remains controversial. In this work, we studied the promotional effect of O-v on photoelectron transfer in TiO2, using first-principles density functional theory calculations with correction for on-site Coulomb interactions. We explicitly identified three types of O-v with different charge states (i.e., charge-neutral , monovalent , divalent O-v(2+)) via electronic structure analysis. Electron transfer energy calculations revealed that the ionized O-v in anatase TiO2 are able to collect excess electrons whereas those in the rutile phase are not. The presence of ionized O-v further endows anatase TiO2 with directional electron transfer along the [100] orientation, in favor of anatase TiO2(101) for photocatalytic reduction surpassing the (001) termination. After examining various combination modes of ionized O-v involving different charge states and spatial distributions, we demonstrated that the vertical chain in anatase TiO2(101) is the most catalytically effective O-v pattern in TiO2. These results signify the importance of subtle defects in photocatalysis and may assist future photocatalyst design toward higher photocatalytic efficiency.
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